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arXiv:1505.07152

Tuning long-range interactions in Sr Rydberg atoms: the effect of series perturbations

Türker Topçu, Andrei Derevianko

Published May 26, 2015• 1 citation
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Abstract

We investigate the effect of series perturbation on the second-order dipole-dipole interactions between strontium atoms in the $5sns({^1}S_0)$ and $5snp({^1}P_1)$ Rydberg states as a means of engineering long-range interactions between atoms. The series perturbation in these atoms enables modifying the strength and the sign of the interaction by varying the principal quantum number $n$ of the Rydberg electron. We utilize experimentally available data to estimate the importance of perturber states, and find that van der Waals interaction between two strontium atoms in the $5snp({^1}P_1)$ states shows strong peaks outside the anticipated hydrogenic $n^{11}$ scaling. We identify this to be the result of the perturbation of $5snd({^1}D_2)$ intermediate states by the $4d^2({^1}D_2)$ and $4dn's({^1}D_2)$ states in the $n<20$ range. This demonstrates that divalent atoms offer a unique advantage for generating substantially stronger or weaker inter-atomic interactions than those that can be achieved using alkali metal atoms. This is due to the highly perturbed spectra of divalent atoms and other multivalent atoms that can persist up to high $n$. Such irregularities can be especially useful in engineering asymmetric Ry blockade requiring the simultaneous presence of both ``weak'' and ``strong'' interactions.

DOI
10.48550/arxiv.1505.07152

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We investigate the effect of series perturbation on the second-order dipole-dipole interactions between strontium atoms in the 5sns(1S0)5sns({^1}S_0)5sns(1S0​) and 5snp(1P1)5snp({^1}P_1)5snp(1P1​) Rydberg states as a means of engineering long-range interactions between atoms. The series perturbation in these atoms enables modifying the strength and the sign of the interaction by varying the principal quantum number nnn of the Rydberg electron. We utilize experimentally available data to estimate the importance of perturber states, and find that van der Waals interaction between two strontium atoms in the 5snp(1P1)5snp({^1}P_1)5snp(1P1​) states shows strong peaks outside the anticipated hydrogenic n11n^{11}n11 scaling. We identify this to be the result of the perturbation of 5snd(1D2)5snd({^1}D_2)5snd(1D2​) intermediate states by the 4d2(1D2)4d^2({^1}D_2)4d2(1D2​) and 4dn′s(1D2)4dn's({^1}D_2)4dn′s(1D2​) states in the n<20n<20n<20 range. This demonstrates that divalent atoms offer a unique advantage for generating substantially stronger or weaker inter-atomic interactions than those that can be achieved using alkali metal atoms. This is due to the highly perturbed spectra of divalent atoms and other multivalent atoms that can persist up to high nnn. Such irregularities can be especially useful in engineering asymmetric Ry blockade requiring the simultaneous presence of both weak'' and strong'' interactions.
We investigate the effect of series perturbation on the second order dipole-dipole interactions between strontium atoms in 5sns(1S0)5sns({^1}S_0)5sns(1S0​) and 5snp(1P1)5snp({^1}P_1)5snp(1P1​) Rydberg states as a means of engineering long-range interactions between atoms in a way that gives an exceptional level of control over the strength and the sign of the interaction by changing nnn. We utilize experimentally available data to estimate the importance of perturber states at low nnn, and find that van der Waals interaction between two strontium atoms in the 5snp(1P1)5snp({^1}P_1)5snp(1P1​) states shows strong peaks outside the usual hydrogenic n11n^{11}n11 scaling. We identify this to be the result of the perturbation of 5snd(1D2)5snd({^1}D_2)5snd(1D2​) intermediate states by the 4d2(1D2)4d^2({^1}D_2)4d2(1D2​) and 4dn′s(1D2)4dn's({^1}D_2)4dn′s(1D2​) states in the n<20n<20n<20 range. This demonstrates that divalent atoms in general present a unique advantage for creating substantially stronger or weaker interaction strengths than those can be achieved using alkali metal atoms due to their highly perturbed spectra that can persist up to high-nnn.
We present calculations of long-range interactions in Rydberg atoms, with a focus on the dipole-dipole interactions of strontium Rydberg states. The growing use of Rydberg states in the field of cold atoms necessitates a more detailed understanding of the effects of dipole-dipole interactions, which are currently being investigated in a number of research groups worldwide. Calculations of long-range interactions in Rydberg states of caesium, cal- cium, rubidium, strontium and ytterbium are presented. By taking the one active electron approximation we develop consistent models of these long- range interactions, and construct a survey of the Rydberg state dipole-dipole interactions and quadrupole-quadrupole interactions. We compare the inter- actions between series and between atoms, highlighting the importance of certain series for applications suggested in previous works. In order to include two-electron effects in the description of dipole-dipole interactions in divalent atoms, we use multichannel quantum defect theory (MQDT) to develop models of the Rydberg series of strontium. We use an empirical reactance matrix formalism, where the reactance matrix is fitted to reproduce experimentally measured values of the bound state energy levels. Models are found for all series of strontium with L ≤ 3. We extend the MQDT formalism to the description of the natural radiative lifetimes of strontium, where the perturbers are found to have a large quenching effect on these lifetimes. By incorporating the MQDT description of the Rydberg states of strontium into the calculation of dipole-dipole interactions, we find a spin-forbidden two-atom resonance in the 3D2 states of strontium. We consider a one- dimensional lattice of strontium atoms, and find that the internal dynamics of the Rydberg atoms demonstrates spin transport for large lattice spacings and a separation of the spin and total angular momentum dynamics for small lattice spacings. Spin-angular momentum separation (analogous to spin-charge separation in condensed matter) in strontium Rydberg atoms may have uses in the investigation of one-dimensional Fermi gases and their description using Luttinger liquid theory.
The production of very-high-nnn ($n\ensuremath{\sim}300$--500) strontium Rydberg atoms is explored using a crossed-laser-atom-beam geometry. nnn1S0{}^{1}{S}_{0}1S0​ and nnn1D2{}^{1}{D}_{2}1D2​ states are created by two-photon excitation via the 5s5p5s5p5s5p 1P1{}^{1}{P}_{1}1P1​ intermediate state using radiation with wavelengths of $\ensuremath{\sim}$461 and $\ensuremath{\sim}$413 nm. Rydberg atom densities as high as $\ensuremath{\sim}3\ifmmode\times\else\texttimes\fi{}{10}^{5}$ cm${}^{\ensuremath{-}3}$ have been achieved, sufficient that Rydberg-Rydberg interactions can become important. The isotope shifts in the Rydberg series limits are determined by tuning the 461-nm light to preferentially excite the different strontium isotopes. Photoexcitation in the presence of an applied electric field is examined. The initially quadratic Stark shift of the nnn1P1{}^{1}{P}_{1}1P1​ and nnn1D2{}^{1}{D}_{2}1D2​ states becomes near-linear at higher fields and the possible use of n1D2n{}^{1}{D}_{2}n1D2​ states to create strongly polarized, quasi-one-dimensional electronic states in strontium is discussed. The data are analyzed with the aid of a two-active-electron (TAE) approximation. The two-electron Hamiltonian, within which the Sr2+{}^{2+}2+ core is represented by a semi-empirical potential, is numerically diagonalized allowing the calculation of the energies of high-nnn Rydberg states and their photoexcitation probabilities.
Quantum information processing with neutral atoms relies on Rydberg excitation for entanglement generation. While the use of heavy divalent or open-shell elements, such as strontium or ytterbium, has benefits due to their optically active core and a variety of possible qubit encodings, their Rydberg structure is generally complex. For some isotopes in particular, hyperfine interactions are relevant even for highly excited electronic states. We employ multichannel quantum defect theory to infer the Rydberg structure of isotopes with nonzero nuclear spin and perform nonperturbative Rydberg-pair interaction calculations. We find that due to the high level density and sensitivities to external fields, experimental parameters must be precisely controlled. Specifically in Sr 87 , we study an intrinsic Förster resonance, unique to divalent atoms with hyperfine-split thresholds, which simultaneously provides line stability with respect to external field fluctuations and enhanced long-range interactions. Additionally, we provide parameters for pair states that can be effectively described by single-channel Rydberg series. The explored pair states provide exciting opportunities for applications in the blockade regime, as well as for more exotic long-range interactions such as largely flat, distance-independent potentials. Published by the American Physical Society 2024
We use perturbation theory to directly calculate the van der Waals and dipole-dipole energy shifts of pairs of interacting Rb Rydberg atoms for different quantum numbers nnn, $\ensuremath{\ell}$, jjj, and mj{m}_{j}mj​, taking into account a large number of perturbing states. Our results can be used to identify good experimental parameters and illuminate important considerations for applications of the ``Rydberg-excitation blockade.'' We also use the results of the calculation to explain features of previous experimental data on the Rydberg-excitation blockade. To explore control methods for the blockade, we discuss energy shifts due to atom-atom interaction in an external electric field.
Abstract Long-range dipole–dipole and quadrupole–quadrupole interactions between pairs of Rydberg atoms are calculated perturbatively for calcium, strontium and ytterbium within the Coulomb approximation. Quantum defects, obtained by fitting existing laser spectroscopic data, are provided for all S, P, D and F series of strontium and for the 3P2 series of calcium. The results show qualitative differences with the alkali metal atoms, including isotropically attractive interactions of the strontium 1S0 states and a greater rarity of Förster resonances. Only two such resonances are identified, both in triplet series of strontium. The angular dependence of the long-range interaction is briefly discussed.